Spin-defect characteristics of single sulfur vacancies in monolayer MoS2

Alexander Hötger; Tomer Amit; Julian Klein; Katja Barthelmi; Thomas Pelini; Alex Delhomme; Sergio Rey; Marek Potemski; Clément Faugeras; Galit Cohen; Daniel Hernangómez-Pérez; Takashi Taniguchi; Kenji Watanabe; Christoph Kastl; Jonathan J Finley; Sivan Refaely-Abramson; Alexander W Holleitner; Andreas V Stier

doi:10.1038/s41699-023-00392-2

Spin-defect characteristics of single sulfur vacancies in monolayer MoS₂

Alexander Hötger, Tomer Amit, Julian Klein, Katja Barthelmi, Thomas Pelini, Alex Delhomme, Sergio Rey, Marek Potemski, Clément Faugeras, Galit Cohen, Daniel Hernangómez-Pérez, Takashi Taniguchi, Kenji Watanabe, Christoph Kastl, Jonathan J Finley, Sivan Refaely-Abramson, Alexander W Holleitner, Andreas V Stier

Weizmann Institute of Science

Research output: Contribution to journal › Article › peer-review

Abstract

Single spin-defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2, and Q*) of He-ion induced sulfur vacancies in monolayer MoS₂. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wave function extent of ~3.5 nm. The distinct valley-Zeeman splitting in out-of-plane B-fields and the brightening of dark states through in-plane B-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.

Original language	English
Article number	30
Journal	npj 2D Materials and Applications
Volume	7
DOIs	https://doi.org/10.1038/s41699-023-00392-2
State	Published - 8 Apr 2023

All Science Journal Classification (ASJC) codes

General Chemistry
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering
General Materials Science

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Hötger, A., Amit, T., Klein, J., Barthelmi, K., Pelini, T., Delhomme, A., Rey, S., Potemski, M., Faugeras, C., Cohen, G., Hernangómez-Pérez, D., Taniguchi, T., Watanabe, K., Kastl, C., Finley, J. J., Refaely-Abramson, S., Holleitner, A. W., & Stier, A. V. (2023). Spin-defect characteristics of single sulfur vacancies in monolayer MoS₂. npj 2D Materials and Applications, 7, Article 30. https://doi.org/10.1038/s41699-023-00392-2

@article{22f737888dd7445eadba42f75193466e,

title = "Spin-defect characteristics of single sulfur vacancies in monolayer MoS2",

abstract = "Single spin-defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2, and Q*) of He-ion induced sulfur vacancies in monolayer MoS2. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wave function extent of ~3.5 nm. The distinct valley-Zeeman splitting in out-of-plane B-fields and the brightening of dark states through in-plane B-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.",

author = "Alexander H{\"o}tger and Tomer Amit and Julian Klein and Katja Barthelmi and Thomas Pelini and Alex Delhomme and Sergio Rey and Marek Potemski and Cl{\'e}ment Faugeras and Galit Cohen and Daniel Hernang{\'o}mez-P{\'e}rez and Takashi Taniguchi and Kenji Watanabe and Christoph Kastl and Finley, {Jonathan J} and Sivan Refaely-Abramson and Holleitner, {Alexander W} and Stier, {Andreas V}",

note = "The work was supported by Deutsche Forschungsgemeinschaft (DFG). We gratefully acknowledge financial support of the German Excellence Initiative by MCQST (EXS-2111) and e-conversion (EXS-2089). This work has been partially supported by the EC Graphene Flagship project and by ANR projects ANR-17-CE24-030 and ANR-19-CE09-0026. This work was supported by LNCMI-CNRS, members of the European Magnetic Field Laboratory (EMFL). J.K. acknowledges support by the Alexander von Humboldt foundation. K.W. and T.T. acknowledge support from the JSPS KAKENHI (Grant Numbers 19H05790, 20H00354 and 21H05233). T.A, G.C., D.H., and S.R-A. acknowledge support from the David Lopatie Fellows Program and the ERC Starting grant 101041159. S.R. acknowledges support from the Independent Research Fund Denmark. AUTHOR CONTRIBUTIONS A.H., J.K., J.J.F., A.W.H., and A.S. conceived and designed the experiments. T.A, G.C., D.H., and S.RA. performed the DFT-GW and BSE calculations. S.R., J.K. prepared the sample. K.W. and T.T. provided highquality hBN bulk crystals. A.H., A.S., T.P., A.D., C.F., J.K. and K.B. performed the optical measurements. A.H. analyzed the data. C.K., M.P. and C.F. contributed interpreting the data. A.H. and A.S. wrote the manuscript with input from all coauthors.",

year = "2023",

month = apr,

day = "8",

doi = "10.1038/s41699-023-00392-2",

language = "الإنجليزيّة",

volume = "7",

journal = "npj 2D Materials and Applications",

issn = "2397-7132",

publisher = "Nature Publishing Group",

}

Hötger, A, Amit, T, Klein, J, Barthelmi, K, Pelini, T, Delhomme, A, Rey, S, Potemski, M, Faugeras, C, Cohen, G, Hernangómez-Pérez, D, Taniguchi, T, Watanabe, K, Kastl, C, Finley, JJ, Refaely-Abramson, S, Holleitner, AW & Stier, AV 2023, 'Spin-defect characteristics of single sulfur vacancies in monolayer MoS₂', npj 2D Materials and Applications, vol. 7, 30. https://doi.org/10.1038/s41699-023-00392-2

TY - JOUR

T1 - Spin-defect characteristics of single sulfur vacancies in monolayer MoS2

AU - Hötger, Alexander

AU - Amit, Tomer

AU - Klein, Julian

AU - Barthelmi, Katja

AU - Pelini, Thomas

AU - Delhomme, Alex

AU - Rey, Sergio

AU - Potemski, Marek

AU - Faugeras, Clément

AU - Cohen, Galit

AU - Hernangómez-Pérez, Daniel

AU - Taniguchi, Takashi

AU - Watanabe, Kenji

AU - Kastl, Christoph

AU - Finley, Jonathan J

AU - Refaely-Abramson, Sivan

AU - Holleitner, Alexander W

AU - Stier, Andreas V

N1 - The work was supported by Deutsche Forschungsgemeinschaft (DFG). We gratefully acknowledge financial support of the German Excellence Initiative by MCQST (EXS-2111) and e-conversion (EXS-2089). This work has been partially supported by the EC Graphene Flagship project and by ANR projects ANR-17-CE24-030 and ANR-19-CE09-0026. This work was supported by LNCMI-CNRS, members of the European Magnetic Field Laboratory (EMFL). J.K. acknowledges support by the Alexander von Humboldt foundation. K.W. and T.T. acknowledge support from the JSPS KAKENHI (Grant Numbers 19H05790, 20H00354 and 21H05233). T.A, G.C., D.H., and S.R-A. acknowledge support from the David Lopatie Fellows Program and the ERC Starting grant 101041159. S.R. acknowledges support from the Independent Research Fund Denmark. AUTHOR CONTRIBUTIONS A.H., J.K., J.J.F., A.W.H., and A.S. conceived and designed the experiments. T.A, G.C., D.H., and S.RA. performed the DFT-GW and BSE calculations. S.R., J.K. prepared the sample. K.W. and T.T. provided highquality hBN bulk crystals. A.H., A.S., T.P., A.D., C.F., J.K. and K.B. performed the optical measurements. A.H. analyzed the data. C.K., M.P. and C.F. contributed interpreting the data. A.H. and A.S. wrote the manuscript with input from all coauthors.

PY - 2023/4/8

Y1 - 2023/4/8

N2 - Single spin-defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2, and Q*) of He-ion induced sulfur vacancies in monolayer MoS2. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wave function extent of ~3.5 nm. The distinct valley-Zeeman splitting in out-of-plane B-fields and the brightening of dark states through in-plane B-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.

AB - Single spin-defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2, and Q*) of He-ion induced sulfur vacancies in monolayer MoS2. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wave function extent of ~3.5 nm. The distinct valley-Zeeman splitting in out-of-plane B-fields and the brightening of dark states through in-plane B-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.

UR - http://www.scopus.com/inward/record.url?scp=85151334138&partnerID=8YFLogxK

U2 - 10.1038/s41699-023-00392-2

DO - 10.1038/s41699-023-00392-2

M3 - مقالة

SN - 2397-7132

VL - 7

JO - npj 2D Materials and Applications

JF - npj 2D Materials and Applications

M1 - 30

ER -

Spin-defect characteristics of single sulfur vacancies in monolayer MoS₂

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